Sub-molecular structural relaxation at a physisorbed interface with monolayer organic single-crystal semiconductors

Yamamura, Akifumi; Fujii, Hiromasa; Ogasawara, Hirohito; Nordlund, Dennis; Takahashi, Osamu; Kishi, Yuutaro; Ishii, Hiroyuki; Kobayashi, Nobuhiko; Niitsu, Naoyuki; Blülle, Balthasar; Okamoto, Toshihiro; Wakabayashi, Yusuke; Watanabe, Shun; Takeya, Jun

doi:10.1038/s42005-020-0285-7

Title: Sub-molecular structural relaxation at a physisorbed interface with monolayer organic single-crystal semiconductors

Journal Article · 22 January 2020 · Communications Physics

DOI: https://doi.org/10.1038/s42005-020-0285-7 · OSTI ID:1605375

Yamamura, Akifumi ^[1]; Fujii, Hiromasa ^[2];

^[3];

^[4]; Kishi, Yuutaro ^[5];

^[5];

^[5]; Niitsu, Naoyuki ^[6]; Blülle, Balthasar ^[6]; Okamoto, Toshihiro ^[1]; Wakabayashi, Yusuke ^[7]; Watanabe, Shun ^[1]; Takeya, Jun ^[1]

Univ. of Tokyo (Japan). Dept. of Advanced Material Science; National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
Osaka Univ. (Japan); Tohoku Univ., Sendai (Japan). Dept. of Physics
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Hiroshima Univ. (Japan). Dept. of Chemistry
Univ. of Tsukuba (Japan)
Univ. of Tokyo (Japan). Dept. of Advanced Material Science
Tohoku Univ., Sendai (Japan). Dept. of Physics

Arranging molecules into highly symmetric, topological crystal structures has been recognized as the best approach to functionalize electronic properties in molecular crystals, where the constituent molecules have been assumed to be rigid in shape. Here, in striking contrast, we demonstrate that the molecules in a monolayer organic crystal can undergo a significant deformation in proximity to the substrate, which is reflected by an asymmetry in the electron density profile. X-ray reflectivity and X-ray absorption spectroscopies in conjunction with density-functional theory calculations reveal that the highly planarized π-core are deformed into a bent shape, while the bulk lattice parameters are maintained. The molecular shape change is found to be perfectly suppressed in a bilayer single crystal, which leads to a 40% increase in mobility in the bilayer crystal. Our finding of a unique, sub-molecular scale shape change in monolayer single crystals can offer possibilities for functionalizing electrical properties via nano-scale physisorption.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1605375

Journal Information:: Communications Physics, Journal Name: Communications Physics Journal Issue: 1 Vol. 3; ISSN 2399-3650

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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